The behaviour of OH* in aqueous environments, nucleation of gas hydrates, and ordering processes in MOFs: insights from molecular simulations

分子模拟已经成为非常强大的工具，它正在极大地影响我们在分子水平上对物质的理解。使用这种方法，我们可以研究相互作用和进化的分子集合，从而提供新的科学见解。我研究的总体目的是探索液体和固体系统的微观行为，以便进一步了解它们的各种化学和物理性质，以及它们在其中的转化和反应。这项建议集中在两个关键领域，一个旨在探索重要类别材料的结晶和有序过程，另一个集中于研究关键的高活性化学物种--羟基自由基在各种水环境中的行为。例如，这项工作将提高我们对冰、天然气水合物和金属有机骨架材料可能形成的方式和时间的基本理解。它还可能最终导致新的方法来抑制天然气水合物在管道中的堵塞，或者控制与羟基自由基有关的疾病，如癌症和衰老。这项研究的结果有可能产生广泛的影响，例如，导致卫生保健结果的改善，更有效和更有效的废水处理，更好的气候模型提供更好的天气预报，以及获得目前储存在大量天然气水合物中的巨大能源财富。 我们的工作将继续建立在我们在几个领域使用分子模拟方面的既定领导地位的基础上，这些领域现在似乎有可能取得重大进展。成核和晶体形成和生长的基础过程将仍然是我们研究的重点领域，基于我们的专业知识和经验，我们将探索分子排列及其动力学，以表征关键结构和事件，以及它们在这些有序化过程中的作用。气体笼状水合物、冰和金属有机骨架(MOF)，这些具有广泛兴趣和重要性的材料，将是我们关注的主要焦点。我们最近扩展到的另一个具有挑战性的领域是对凝聚相中的羟基自由基(OH*)的分子模拟，并在其中取得了重大进展。我们将探索这一关键化学物种在不同水环境中(例如，水或冰的内部或表面)的局部结构及其影响，在那里我们将探索OH*与各种对大气和生化环境重要的小分子的相互作用和反应。多尺度建模方法将是这项工作许多方面的共同主题。我们将继续开拓新的分析和可视化工具，使我们能够从所执行的模拟中获得更多的见解(除了目前可用的)，从而使我们对这些系统和流程的理解取得重大进展。

Molecular simulations have become very powerful tools that are dramatically impacting our understanding of matter at the molecular level. Using such approaches, we can examine collections of molecules interacting and evolving thereby providing new scientific insights. The overall aim of my research is to probe the microscopic behaviour of liquid and solid systems in order to further our understanding of their various chemical and physical properties, their transformations and reactions within them. This proposal focuses on two key areas, one aimed at exploring crystallization and ordering processes for important classes of materials, and the other centered on investigating the behaviour of a key and highly reactive chemical species, the hydroxyl radical, in various aqueous environments. This work will improve our fundamental understanding of, for example, how and when ice, gas hydrates and metal-organic framework materials may form. It may also eventually lead to new ways to inhibit gas hydrate plugs in pipelines or to control diseases that have links to the hydroxyl radical, such as cancer and aging. The results of this research have potential for broad impact by leading to, for example, improved health-care outcomes, more efficient and effective wastewater treatments, better climate models providing improved weather forecasts, and access to the enormous energy wealth currently stored in vast reserves of natural gas hydrates. Our work will continue to build on our established leadership in using molecular simulations in several areas, where significant advances now appear possible. Nucleation and the processes underlying the formation and growth of crystals will remain an area of focus of our research, building upon our expertise and experience, where molecular arrangement and their dynamics will be probed in order to characterize key structures and events, and their roles within these ordering processes. Gas clathrate hydrates, ice and metal-organic frameworks (MOFs), materials of broad interest and importance, will be primary focuses of our attention. Another challenging area we have recently expanded into, and made significant advances within, is the molecular simulations of the hydroxyl radical (OH*) in condensed phases. The local structure and its impacts for this key chemical species in various aqueous environments (e.g. within, or on the surfaces of, water or ice) will be explored, where we will probe the interactions and reactions of OH* with various small molecules important to atmospheric and biochemical contexts. Multiscale modeling approaches will be a common theme across many aspects of this work. We will continue to pioneer new analysis and visualization tools to allow us to gain additional insights (beyond those currently available) from the simulations performed, thereby allowing for significant advances to our understanding of these systems and processes.